Thermally Reprocessable Self-Healing Single-Ion Conducting Polymer Electrolytes

Self-healing polymer electrolytes are essential for overcoming the limitations of liquid and solid electrolytes by offering superior mechanical robustness, enhanced safety, and repeated processability. Herein, we present thermally reprocessable and self-healing thermosets for solid polymer electrolytes using sulfonylimide-based anionic monomers and thermo-reversible Diels-Alder chemistry. Six different types of linear copolymers are synthesized by varying the chemical structures of furan-containing monomers and the proportion of electrolytic components. Then, bismaleimide cross-linkers are introduced to form thermally reversible cross-linked networks. We investigate the effect of the comonomer ratio and monomer structure on the thermomechanical and electrochemical properties of these polymers. Furthermore, we evaluate the mechanical and ion conducting properties after up to 30 thermal reprocessing cycles. Our findings demonstrate the potential of these thermosets as promising candidates for high-performance solid polymer electrolytes in lithium-ion batteries.